Hydrogen production by molecular photocatalysis

被引:1292
作者
Esswein, Arthur J. [1 ]
Nocera, Daniel G. [1 ]
机构
[1] MIT, Dept Chem 6335, Cambridge, MA 02139 USA
关键词
D O I
10.1021/cr050193e
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Hydrogen can be produced by means of molecular photocatalysis from RH dehydrogenations. This is where the proton and electron equivalents for H2 production originate from C-H or O-H bonds. The most well-defined schemes for photocatalytic H2 production is alkane dehydrogenation, which happens by classical organometallic mechanisms involving alkane C-H bond activation. An alternative photocatalytic route is through mercury photosensitization of the dehydrodimerization of alkanes and was made viable for the formation of C-C bonds. Another is alcohol photo-dehydrogenation to ketones or aldehydes. They are not limited to late transition metal centers and can open a coordination site to support a two-electron oxidation state change to generate H2. A recent technique involves catalytically dehydrogenate NADH analogs in anaerobic acetonitrile solution under irradiation. H2 can also be produced from low-energy substrates directly such as acids. In order to enrich the hydrogen content in water gas after the steam reforming of methane, photochemical water-gas shift are widely used in industry. In a three-component system, the scheme is composed of one-electron photosensitizer, a redox mediator and the redox-storing catalyst. Another is through photobiological approaches to H2 production and is depended on th activity of photosynthetic organisms or the enzymatic activity of hydrogenase. It can be done through the activity of hydrogenase or isolated chloroplasts.
引用
收藏
页码:4022 / 4047
页数:26
相关论文
共 413 条
[31]   DYE-SENSITIZED PHOTOREDUCTION OF METHYL VIOLOGEN [J].
BELLIN, JS ;
ALEXANDER, R ;
MAHONEY, RD .
PHOTOCHEMISTRY AND PHOTOBIOLOGY, 1973, 17 (01) :17-24
[32]   Organometallic photochemistry at the end of its first century [J].
Bitterwolf, TE .
JOURNAL OF ORGANOMETALLIC CHEMISTRY, 2004, 689 (24) :3939-3952
[33]   Cooperative bimetallic redox reactivity [J].
Bosnich, B .
INORGANIC CHEMISTRY, 1999, 38 (11) :2554-2562
[34]   ELECTRONIC SPECTRAL STUDIES OF PLANAR RHODIUM(I) AND IRIDIUM(I) COMPLEXES CONTAINING PI-ACCEPTOR LIGANDS [J].
BRADY, R ;
FLYNN, BR ;
GEOFFROY, GL ;
GRAY, HB ;
PEONE, J ;
VASKA, L .
INORGANIC CHEMISTRY, 1976, 15 (07) :1485-1488
[35]   MECHANISM OF THE FORMATION OF DIHYDROGEN FROM THE PHOTOINDUCED REACTIONS OF TRIS(BIPYRIDINE)RUTHENIUM(II) WITH TRIS(BIPYRIDINE)RHODIUM(III) [J].
BROWN, GM ;
CHAN, SF ;
CREUTZ, C ;
SCHWARZ, HA ;
SUTIN, N .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1979, 101 (25) :7638-7640
[36]   A NOVEL ROUTE TO ALKANES, ALCOHOLS, AND ETHERS BY DEHYDRODIMERIZATION [J].
BROWN, SH ;
CRABTREE, RH .
TETRAHEDRON LETTERS, 1987, 28 (46) :5599-5602
[37]   MAKING MERCURY-PHOTOSENSITIZED DEHYDRODIMERIZATION INTO AN ORGANIC SYNTHETIC METHOD - VAPOR-PRESSURE SELECTIVITY AND THE BEHAVIOR OF FUNCTIONALIZED SUBSTRATES [J].
BROWN, SH ;
CRABTREE, RH .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1989, 111 (08) :2935-2946
[38]   ALKANE FUNCTIONALIZATION ON A PREPARATIVE SCALE BY MERCURY-PHOTOSENSITIZED CROSS-DEHYDRODIMERIZATION [J].
BROWN, SH ;
CRABTREE, RH .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1989, 111 (08) :2946-2953
[39]   PHOTOREDOX REACTIONS IN FUNCTIONAL MICELLAR ASSEMBLIES - USE OF AMPHIPHILIC REDOX RELAYS TO ACHIEVE LIGHT ENERGY-CONVERSION AND CHARGE SEPARATION [J].
BRUGGER, PA ;
INFELTA, PP ;
BRAUN, AM ;
GRATZEL, M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1981, 103 (02) :320-326
[40]   Mechanism of molybdenum nitrogenase [J].
Burgess, BK ;
Lowe, DJ .
CHEMICAL REVIEWS, 1996, 96 (07) :2983-3011